Full on-device manipulation of olefin metathesis for precise manufacturing

IF 38.1 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Nature nanotechnology Pub Date : 2024-11-08 DOI:10.1038/s41565-024-01814-y
Yilin Guo, Chen Yang, Lei Zhang, Yujie Hu, Jie Hao, Chuancheng Jia, Yang Yang, Yan Xu, Xingxing Li, Fanyang Mo, Yanwei Li, Kendall N. Houk, Xuefeng Guo
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Abstract

Olefin metathesis, as a powerful metal-catalysed carbon–carbon bond-forming method, has achieved considerable progress in recent years. However, the complexity originating from multicomponent interactions has long impeded a complete mechanistic understanding of olefin metathesis, which hampers further optimization of the reaction. Here, we clarify both productive and hidden degenerate pathways of ring-closing metathesis by focusing on one individual catalyst, using a sensitive single-molecule electrical detection platform. In addition to visualizing the full pathway, we found that the conventionally unwanted degenerate pathways have an unexpected constructive coupling effect on the productive pathway, and both types of pathway can be regulated by an external electric field. We then pushed forward this ability to ring-opening metathesis polymerization involving more interactive components. With single-monomer-insertion-event resolution, precise on-device synthesis of a single polymer was achieved by online manipulation of monomer insertion dynamics, intramolecular chain transfer, stereoregularity, degree of polymerization and block copolymerization. These results offer a comprehensive mechanistic understanding of olefin metathesis, exemplifying infinite opportunities for practical precise manufacturing.

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完全在设备上操纵烯烃偏析,实现精确制造
烯烃偏聚反应作为一种功能强大的金属催化碳碳键形成方法,近年来取得了长足的进步。然而,长期以来,多组分相互作用产生的复杂性阻碍了人们对烯烃偏聚反应的完整机理理解,从而妨碍了该反应的进一步优化。在这里,我们利用灵敏的单分子电学检测平台,以单个催化剂为研究对象,阐明了闭环复分解反应的生产途径和隐藏的退化途径。除了可视化整个途径外,我们还发现传统上不受欢迎的退化途径对生产性途径具有意想不到的建设性耦合效应,而且这两种途径都可以通过外部电场进行调节。随后,我们将这种能力推进到涉及更多交互成分的开环偏聚聚合反应中。通过在线操纵单体插入动力学、分子内链转移、立体规整度、聚合度和嵌段共聚,以单单体插入事件为分辨率,在设备上实现了单个聚合物的精确合成。这些结果提供了对烯烃偏聚作用的全面机械理解,为实际的精确制造提供了无限机会。
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来源期刊
Nature nanotechnology
Nature nanotechnology 工程技术-材料科学:综合
CiteScore
59.70
自引率
0.80%
发文量
196
审稿时长
4-8 weeks
期刊介绍: Nature Nanotechnology is a prestigious journal that publishes high-quality papers in various areas of nanoscience and nanotechnology. The journal focuses on the design, characterization, and production of structures, devices, and systems that manipulate and control materials at atomic, molecular, and macromolecular scales. It encompasses both bottom-up and top-down approaches, as well as their combinations. Furthermore, Nature Nanotechnology fosters the exchange of ideas among researchers from diverse disciplines such as chemistry, physics, material science, biomedical research, engineering, and more. It promotes collaboration at the forefront of this multidisciplinary field. The journal covers a wide range of topics, from fundamental research in physics, chemistry, and biology, including computational work and simulations, to the development of innovative devices and technologies for various industrial sectors such as information technology, medicine, manufacturing, high-performance materials, energy, and environmental technologies. It includes coverage of organic, inorganic, and hybrid materials.
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